From Fundamental Theories to Quantum Coherences in Electron Transfer

Shahnawaz Rafiq, Gregory D. Scholes

Research output: Contribution to journalReview article

22 Scopus citations

Abstract

Photoinduced electron transfer (ET) is a cornerstone of energy transduction from light to chemistry. The past decade has seen tremendous advances in the possible role of quantum coherent effects in the light-initiated energy and ET processes in chemical, biological, and materials systems. The prevalence of such coherence effects holds a promise to increase the efficiency and robustness of transport even in the face of energetic or structural disorder. A primary motive of this Perspective is to work out how to think about "coherence" in ET reactions. We will discuss how the interplay of basic parameters governing ET reactions - like electronic coupling, interactions with the environment, and intramolecular high-frequency quantum vibrations - impact coherences. This includes revisiting the insights from the seminal work on the theory of ET and time-resolved measurements on coherent dynamics to explore the role of coherences in ET reactions. We conclude by suggesting that in addition to optical spectroscopies, validating the functional role of coherences would require simultaneous mapping of correlated electron motion and atomically resolved nuclear structure. ©

Original languageEnglish (US)
Pages (from-to)708-722
Number of pages15
JournalJournal of the American Chemical Society
Volume141
Issue number2
DOIs
StatePublished - Jan 16 2019

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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